US10826121B2 - Electrolyte and secondary battery - Google Patents
Electrolyte and secondary battery Download PDFInfo
- Publication number
- US10826121B2 US10826121B2 US15/891,197 US201815891197A US10826121B2 US 10826121 B2 US10826121 B2 US 10826121B2 US 201815891197 A US201815891197 A US 201815891197A US 10826121 B2 US10826121 B2 US 10826121B2
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- US
- United States
- Prior art keywords
- electrolyte
- additive
- carbonate
- secondary battery
- lithium
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 110
- 239000000654 additive Substances 0.000 claims abstract description 63
- 230000000996 additive effect Effects 0.000 claims abstract description 63
- YZYDPPZYDIRSJT-UHFFFAOYSA-K boron phosphate Chemical group [B+3].[O-]P([O-])([O-])=O YZYDPPZYDIRSJT-UHFFFAOYSA-K 0.000 claims abstract description 41
- 229910000149 boron phosphate Inorganic materials 0.000 claims abstract description 41
- 239000011356 non-aqueous organic solvent Substances 0.000 claims abstract description 23
- 150000003839 salts Chemical class 0.000 claims abstract description 11
- -1 cyclic carbonate ester Chemical class 0.000 claims description 19
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 claims description 9
- 150000001875 compounds Chemical class 0.000 claims description 7
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 claims description 6
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 6
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 6
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 claims description 6
- 125000003342 alkenyl group Chemical group 0.000 claims description 6
- 125000000217 alkyl group Chemical group 0.000 claims description 6
- 125000000304 alkynyl group Chemical group 0.000 claims description 6
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 6
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 claims description 6
- TZIHFWKZFHZASV-UHFFFAOYSA-N methyl formate Chemical compound COC=O TZIHFWKZFHZASV-UHFFFAOYSA-N 0.000 claims description 6
- 125000003118 aryl group Chemical group 0.000 claims description 5
- 125000005843 halogen group Chemical group 0.000 claims description 5
- UHOPWFKONJYLCF-UHFFFAOYSA-N 2-(2-sulfanylethyl)isoindole-1,3-dione Chemical compound C1=CC=C2C(=O)N(CCS)C(=O)C2=C1 UHOPWFKONJYLCF-UHFFFAOYSA-N 0.000 claims description 3
- LWLOKSXSAUHTJO-UHFFFAOYSA-N 4,5-dimethyl-1,3-dioxolan-2-one Chemical compound CC1OC(=O)OC1C LWLOKSXSAUHTJO-UHFFFAOYSA-N 0.000 claims description 3
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims description 3
- FERIUCNNQQJTOY-UHFFFAOYSA-M Butyrate Chemical compound CCCC([O-])=O FERIUCNNQQJTOY-UHFFFAOYSA-M 0.000 claims description 3
- RJUFJBKOKNCXHH-UHFFFAOYSA-N Methyl propionate Chemical compound CCC(=O)OC RJUFJBKOKNCXHH-UHFFFAOYSA-N 0.000 claims description 3
- KXKVLQRXCPHEJC-UHFFFAOYSA-N acetic acid trimethyl ester Natural products COC(C)=O KXKVLQRXCPHEJC-UHFFFAOYSA-N 0.000 claims description 3
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 3
- VUPKGFBOKBGHFZ-UHFFFAOYSA-N dipropyl carbonate Chemical compound CCCOC(=O)OCCC VUPKGFBOKBGHFZ-UHFFFAOYSA-N 0.000 claims description 3
- 229940093499 ethyl acetate Drugs 0.000 claims description 3
- CYEDOLFRAIXARV-UHFFFAOYSA-N ethyl propyl carbonate Chemical compound CCCOC(=O)OCC CYEDOLFRAIXARV-UHFFFAOYSA-N 0.000 claims description 3
- WBJINCZRORDGAQ-UHFFFAOYSA-N formic acid ethyl ester Natural products CCOC=O WBJINCZRORDGAQ-UHFFFAOYSA-N 0.000 claims description 3
- 229940017219 methyl propionate Drugs 0.000 claims description 3
- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-UHFFFAOYSA-N 0.000 claims description 3
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 claims description 3
- 229940090181 propyl acetate Drugs 0.000 claims description 3
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 3
- NQPDZGIKBAWPEJ-UHFFFAOYSA-N valeric acid Chemical compound CCCCC(O)=O NQPDZGIKBAWPEJ-UHFFFAOYSA-N 0.000 claims description 3
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 73
- 229910001416 lithium ion Inorganic materials 0.000 description 73
- 238000000034 method Methods 0.000 description 25
- 230000000052 comparative effect Effects 0.000 description 24
- 230000008569 process Effects 0.000 description 23
- 238000002360 preparation method Methods 0.000 description 21
- 238000003860 storage Methods 0.000 description 19
- 229910052796 boron Inorganic materials 0.000 description 11
- 230000003247 decreasing effect Effects 0.000 description 11
- 229910019142 PO4 Inorganic materials 0.000 description 10
- 230000014759 maintenance of location Effects 0.000 description 10
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 10
- 239000010452 phosphate Substances 0.000 description 10
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 description 8
- 239000007774 positive electrode material Substances 0.000 description 7
- FSSPGSAQUIYDCN-UHFFFAOYSA-N 1,3-Propane sultone Chemical compound O=S1(=O)CCCO1 FSSPGSAQUIYDCN-UHFFFAOYSA-N 0.000 description 6
- KRHYYFGTRYWZRS-UHFFFAOYSA-N Fluorane Chemical compound F KRHYYFGTRYWZRS-UHFFFAOYSA-N 0.000 description 6
- FPYJFEHAWHCUMM-UHFFFAOYSA-N maleic anhydride Chemical compound O=C1OC(=O)C=C1 FPYJFEHAWHCUMM-UHFFFAOYSA-N 0.000 description 6
- 238000012360 testing method Methods 0.000 description 6
- ZPFAVCIQZKRBGF-UHFFFAOYSA-N 1,3,2-dioxathiolane 2,2-dioxide Chemical compound O=S1(=O)OCCO1 ZPFAVCIQZKRBGF-UHFFFAOYSA-N 0.000 description 5
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 description 5
- BJWMSGRKJIOCNR-UHFFFAOYSA-N 4-ethenyl-1,3-dioxolan-2-one Chemical compound C=CC1COC(=O)O1 BJWMSGRKJIOCNR-UHFFFAOYSA-N 0.000 description 4
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 4
- 239000011149 active material Substances 0.000 description 4
- 150000001733 carboxylic acid esters Chemical class 0.000 description 4
- 238000010668 complexation reaction Methods 0.000 description 4
- 125000004122 cyclic group Chemical group 0.000 description 4
- 239000011267 electrode slurry Substances 0.000 description 4
- 229910052744 lithium Inorganic materials 0.000 description 4
- 238000007086 side reaction Methods 0.000 description 4
- 125000004429 atom Chemical group 0.000 description 3
- 229910003002 lithium salt Inorganic materials 0.000 description 3
- 159000000002 lithium salts Chemical class 0.000 description 3
- 239000012528 membrane Substances 0.000 description 3
- 239000007773 negative electrode material Substances 0.000 description 3
- KAKZBPTYRLMSJV-UHFFFAOYSA-N Butadiene Chemical group C=CC=C KAKZBPTYRLMSJV-UHFFFAOYSA-N 0.000 description 2
- 239000006245 Carbon black Super-P Substances 0.000 description 2
- 229910001290 LiPF6 Inorganic materials 0.000 description 2
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 2
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 2
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 2
- 229910021383 artificial graphite Inorganic materials 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 239000006258 conductive agent Substances 0.000 description 2
- 238000005520 cutting process Methods 0.000 description 2
- 150000003972 cyclic carboxylic anhydrides Chemical class 0.000 description 2
- 238000007599 discharging Methods 0.000 description 2
- 238000004090 dissolution Methods 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 238000003825 pressing Methods 0.000 description 2
- 230000001681 protective effect Effects 0.000 description 2
- 239000002904 solvent Substances 0.000 description 2
- BDHFUVZGWQCTTF-UHFFFAOYSA-M sulfonate Chemical compound [O-]S(=O)=O BDHFUVZGWQCTTF-UHFFFAOYSA-M 0.000 description 2
- 229910052717 sulfur Inorganic materials 0.000 description 2
- 239000011593 sulfur Substances 0.000 description 2
- 229910052723 transition metal Inorganic materials 0.000 description 2
- 150000003624 transition metals Chemical class 0.000 description 2
- 238000009966 trimming Methods 0.000 description 2
- 238000003466 welding Methods 0.000 description 2
- AEPSPPZMRBUGHA-UHFFFAOYSA-N C=CC=C.[B] Chemical group C=CC=C.[B] AEPSPPZMRBUGHA-UHFFFAOYSA-N 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- 239000002879 Lewis base Substances 0.000 description 1
- 229910001560 Li(CF3SO2)2N Inorganic materials 0.000 description 1
- 229910005140 Li(FSO2)2N Inorganic materials 0.000 description 1
- 229910013188 LiBOB Inorganic materials 0.000 description 1
- 229910000552 LiCF3SO3 Inorganic materials 0.000 description 1
- 229910032387 LiCoO2 Inorganic materials 0.000 description 1
- 229910052493 LiFePO4 Inorganic materials 0.000 description 1
- 229910014985 LiMnxFe1-xPO4 Inorganic materials 0.000 description 1
- 229910014982 LiMnxFe1−xPO4 Inorganic materials 0.000 description 1
- 229910001228 Li[Ni1/3Co1/3Mn1/3]O2 (NCM 111) Inorganic materials 0.000 description 1
- 229910000572 Lithium Nickel Cobalt Manganese Oxide (NCM) Inorganic materials 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 1
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 1
- FDLZQPXZHIFURF-UHFFFAOYSA-N [O-2].[Ti+4].[Li+] Chemical compound [O-2].[Ti+4].[Li+] FDLZQPXZHIFURF-UHFFFAOYSA-N 0.000 description 1
- FBDMJGHBCPNRGF-UHFFFAOYSA-M [OH-].[Li+].[O-2].[Mn+2] Chemical compound [OH-].[Li+].[O-2].[Mn+2] FBDMJGHBCPNRGF-UHFFFAOYSA-M 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- NDPGDHBNXZOBJS-UHFFFAOYSA-N aluminum lithium cobalt(2+) nickel(2+) oxygen(2-) Chemical compound [Li+].[O--].[O--].[O--].[O--].[Al+3].[Co++].[Ni++] NDPGDHBNXZOBJS-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- FFBHFFJDDLITSX-UHFFFAOYSA-N benzyl N-[2-hydroxy-4-(3-oxomorpholin-4-yl)phenyl]carbamate Chemical compound OC1=C(NC(=O)OCC2=CC=CC=C2)C=CC(=C1)N1CCOCC1=O FFBHFFJDDLITSX-UHFFFAOYSA-N 0.000 description 1
- NHWZQIYTQZEOSJ-UHFFFAOYSA-N carbonic acid;phosphoric acid Chemical compound OC(O)=O.OP(O)(O)=O NHWZQIYTQZEOSJ-UHFFFAOYSA-N 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 229910021385 hard carbon Inorganic materials 0.000 description 1
- 150000007527 lewis bases Chemical class 0.000 description 1
- 229910001540 lithium hexafluoroarsenate(V) Inorganic materials 0.000 description 1
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 description 1
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 description 1
- 229910001486 lithium perchlorate Inorganic materials 0.000 description 1
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 description 1
- DVATZODUVBMYHN-UHFFFAOYSA-K lithium;iron(2+);manganese(2+);phosphate Chemical compound [Li+].[Mn+2].[Fe+2].[O-]P([O-])([O-])=O DVATZODUVBMYHN-UHFFFAOYSA-K 0.000 description 1
- 230000003446 memory effect Effects 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 239000002153 silicon-carbon composite material Substances 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000011734 sodium Substances 0.000 description 1
- 159000000000 sodium salts Chemical class 0.000 description 1
- 229910021384 soft carbon Inorganic materials 0.000 description 1
- 230000002195 synergetic effect Effects 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 150000003751 zinc Chemical class 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
- 239000011701 zinc Substances 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0569—Liquid materials characterised by the solvents
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
- H01M2300/0028—Organic electrolyte characterised by the solvent
- H01M2300/0037—Mixture of solvents
- H01M2300/004—Three solvents
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Definitions
- the present disclosure relates to the field of battery, and particularly relates to an electrolyte and a secondary battery.
- a lithium-ion secondary battery is a green, high-capacity and environment-friendly battery appeared in the 1990s. Due to advantages, such as high voltage, small volume, light mass, high specific capacity, non-memory effect, non-pollution, small self-discharge and long cycle life, the lithium-ion secondary battery has been widely applied in light, thin, small and multi-functional portable electronic products, such as mobile phones, laptops, video cameras, digital cameras and tablet personal computers.
- the lithium ion secondary battery used as a power supply of an electric vehicle has been rapidly developed.
- the lithium-ion secondary battery In order to meet the requirements of the electric vehicle for long operation time, long endurance mileage, long cycle life, operating properly under both high temperature environment and low temperature environment and enabling fast charging, the lithium-ion secondary battery needs to have higher discharge capacity, higher energy density, more excellent high temperature cycle performance, more excellent high temperature storage performance and more excellent low temperature rate performance.
- the performances of the lithium-ion secondary battery are serious deteriorated.
- an object of the present disclosure is to provide an electrolyte and a secondary battery, when the electrolyte is applied in the secondary battery, performances of the secondary battery under high temperature environment can be effectively improved.
- the present disclosure provides an electrolyte, which comprises: a non-aqueous organic solvent; an electrolyte salt dissolved in the non-aqueous organic solvent; and an additive dissolved in the non-aqueous organic solvent.
- the additive comprises a first additive, the first additive is selected from boron phosphate represented by formula 1.
- the present disclosure provides a secondary battery, which comprises the electrolyte according to the first aspect of the present disclosure.
- the present disclosure has following beneficial effects: in the electrolyte of the present disclosure, oxidation products of the boron phosphate during charging process can form a stable protective membrane on the surface of the active material, therefore side reactions between the electrolyte and the surface of the active material are effectively decreased, the amount of transition metal dissolution of the positive active material is decreased, and high temperature cycle performance and high temperature storage performance of the secondary battery are improved. Moreover, there is a complexation reaction between B atom in the boron phosphate and hydrofluoric acid in the electrolyte, therefore the gas generation amount of the secondary battery after stored under high temperature environment is decreased.
- the electrolyte according to the first aspect of the present disclosure comprises: a non-aqueous organic solvent; an electrolyte salt dissolved in the non-aqueous organic solvent; and an additive dissolved in the non-aqueous organic solvent.
- the additive comprises a first additive, the first additive is selected from boron phosphate represented by formula 1.
- oxidation products of the boron phosphate during charging process can form a stable protective membrane on the surface of the active material, therefore side reactions between the electrolyte and the surface of the active material are effectively decreased, the amount of transition metal dissolution of the positive active material is also decreased, and high temperature cycle performance and high temperature storage performance of the secondary battery are improved.
- the boron phosphate belongs to Lewis base and P ⁇ O in the boron phosphate has lone pair electrons, there is a complexation reaction between the boron phosphate and PF 5 in the electrolyte, therefore reactivity of PF 5 is decreased, probability of occurrence of the side reactions is also decreased, and high temperature cycle performance of the secondary battery is improved.
- there is also a complexation reaction between B atom in the boron phosphate and hydrofluoric acid in the electrolyte therefore the gas generation amount of the secondary battery after stored under high temperature is decreased.
- the additive may further comprise a second additive, the second additive may be one or more selected from a group consisting of sulfur-containing cyclic lactone, C—C double bond-containing cyclic carbonate ester, and cyclic carboxylic anhydride.
- the sulfur-containing cyclic lactone may comprise cyclic sulfate and cyclic sulfonate.
- the cyclic sulfate may be one or more selected from a group consisting of compounds represented by formula 2 to formula 5.
- R 1 ⁇ R 14 are independently selected from a group consisting of H, substituted or unsubstituted C1 ⁇ C10 alkyl, substituted or unsubstituted C2 ⁇ C10 alkenyl, substituted or unsubstituted C2 ⁇ C10 alkynyl and substituted or unsubstituted C6 ⁇ C10 aryl.
- the cyclic sulfonate may be one or more selected from a group consisting of compounds represented by formula 6 to formula 9.
- R 15 ⁇ R 32 are independently selected from a group consisting of H, halogen atom, substituted or unsubstituted C1 ⁇ C10 alkyl, substituted or unsubstituted C2 ⁇ C10 alkenyl, substituted or unsubstituted C2 ⁇ C10 alkynyl and substituted or unsubstituted C6 ⁇ C10
- the C—C double bond-containing cyclic carbonate ester may be one or more selected from a group consisting of compounds represented by formula 10 to formula 19.
- R 33 ⁇ R 57 are independently selected from a group consisting of H, halogen atom, substituted or unsubstituted C1 ⁇ C10 alkyl, substituted or unsubstituted C2 ⁇ C10 alkenyl, substituted or unsubstituted C2 ⁇ C10 alkynyl and substituted or unsubstituted C6 ⁇ C10 aryl.
- the cyclic carboxylic anhydride may be one or more selected from a group consisting of compounds represented by formula 20 and formula 21.
- R 58 ⁇ R 61 each are independently one selected from a group consisting of H, halogen atom, substituted or unsubstituted C1 ⁇ C10 alkyl, substituted or unsubstituted C2 ⁇ C10 alkenyl, substituted or unsubstituted C2 ⁇ C10 alkynyl and substituted or unsubstituted C6 ⁇ C10 aryl.
- the second additive may be one or more selected from a group consisting of the following compounds:
- a mass of the first additive may be 0.01% ⁇ 5% of a total mass of the electrolyte.
- a mass of the second additive may be 0.01% ⁇ 5% of the total mass of the electrolyte.
- a specific type of the non-aqueous organic solvent is not specifically limited and may be selected based on actual demands.
- the non-aqueous organic solvent may comprise conventional carbonate ester and conventional carboxylic acid ester.
- the carbonate ester may comprise cyclic carboxylic acid ester and/or chain carboxylic acid ester.
- the non-aqueous organic solvent comprises: cyclic carbonate ester; and chain carbonate ester and/or a carboxylic acid ester.
- the cyclic carbonate ester may be one or more selected from a group consisting of ethylene carbonate, propylene carbonate, 2,3-butylene carbonate and ⁇ -butyrolactone.
- the chain carbonate ester may be one or more selected from a group consisting of dimethyl carbonate, diethyl carbonate, dipropyl carbonate, ethyl methyl carbonate, methyl propyl carbonate and ethyl propyl carbonate.
- the carboxylic acid ester may be one or more selected from a group consisting of methyl formate, ethyl formate, propyl formate, methyl acetate, ethyl acetate, propyl acetate, methyl propionate, ethyl propionate and propyl propionate.
- the non-aqueous organic solvent may further comprise halogenated carbonate ester.
- the non-aqueous organic solvent may further comprise fluoroethylene carbonate.
- the electrolyte salt may be a lithium salt, a sodium salt or a zinc salt, and the specific type of the electrolyte salt may be changed according to the specific type of the secondary battery.
- a molar concentration of the electrolyte salt in the electrolyte may be 0.01 mol/L ⁇ 3 mol/L.
- the secondary battery according to the second aspect of the present disclosure comprises the electrolyte according to the first aspect of the present disclosure.
- the secondary battery may be a lithium secondary battery, a sodium secondary battery or a zinc secondary battery.
- the lithium secondary battery may be a lithium-ion secondary battery or a metal lithium secondary battery.
- the secondary battery further comprises a positive electrode plate, a negative electrode plate, a separator and a package shell.
- the positive electrode plate comprises a positive current collector and a positive film, the positive film is positioned on the positive current collector, and the positive film comprises a positive active material.
- the negative electrode plate comprises a negative current collector and a negative film, the negative film is positioned on the negative current collector, and the negative film comprises a negative active material.
- the separator is interposed between the positive electrode plate and the negative electrode plate.
- the positive active material may be one or more selected from a group consisting of lithium cobaltate (LiCoO 2 ), lithium manganese dioxide (LiMnO 2 ), lithium nickel cobalt manganese oxide (NCM), lithium nickel cobalt aluminum oxide (NCA), lithium iron phosphate (LiFePO 4 ) and lithium iron manganese phosphate (LiMn x Fe 1-x PO 4 ).
- the negative active material may be one or more selected from a group consisting of natural graphite, artificial graphite, soft carbon, hard carbon, lithium titanium oxide, silicon, and silicon-carbon composite.
- the electrolyte salt (that is the lithium salt) may be one or more selected from a group consisting of Li(FSO 2 ) 2 N, LiPF 6 , LiBF 4 , LiBOB, LiDFOB, LiAsF 6 , Li(CF 3 SO 2 ) 2 N, LiCF 3 SO 3 and LiClO 4 .
- the illustrated secondary battery is a lithium-ion secondary battery, but the present disclosure is not limited.
- a positive electrode plate LiNi 1/3 Co 1/3 Mn 1/3 O 2 (positive active material), Super-P (conductive agent), PVDF (binder) according to a mass ratio of 96:2:2 were uniformly mixed with N-methyl-2-pyrrolidone (solvent) to form a positive electrode slurry, then the positive electrode slurry was uniformly coated on an aluminum foil (positive current collector) with a coating weight of 0.018 g/cm 2 , baking was then performed at 85° C., which was followed by cold pressing, then after edge-trimming, plate cutting, slitting, baking at 85° C. for 4 h under vacuum and welding a tab, the required positive electrode plate was obtained.
- the electrolyte used LiPF 6 with a molar concentration of 1 mol/L as a lithium salt, and used a mixture of ethylene carbonate (EC), ethyl methyl carbonate (EMC) and diethyl carbonate (DEC) as a non-aqueous organic solvent, a mass ratio of EC, EMC and DEC was 30:50:20.
- the electrolyte further contained an additive, the additive was boron phosphate, and a mass of the boron phosphate was 1% of a total mass of the electrolyte.
- the prepared electrolyte was injected and standby for 24 h, which was followed by charging to 4.2 V at a constant current of 0.1 C (160 mA), then charging to 0.05 C (80 mA) at a constant voltage of 4.2 V, then discharging to 3.0 Vat a constant current of 0.1 C (160 mA), the above charging and discharging process were repeated twice, which was followed by charging to 3.8 V at a constant current of 0.1 C (160 mA), and finally the preparation of the lithium-ion secondary battery was completed.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), the additive was boron phosphate, the mass of the boron phosphate was 0.5% of the total mass of the electrolyte.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), the additive was boron phosphate, the mass of the boron phosphate was 3% of the total mass of the electrolyte.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), the additive was boron phosphate, the mass of the boron phosphate was 5% of the total mass of the electrolyte.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), the additive was boron phosphate and ethylene sulfate, the mass of the boron phosphate was 1% of the total mass of the electrolyte, the mass of the ethylene sulfate was 1% of the total mass of the electrolyte.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), the additive was boron phosphate and 1,3-propanesultone, the mass of the boron phosphate was 1% of the total mass of the electrolyte, the mass of the 1,3-propanesultone was 1% of the total mass of the electrolyte.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), the additive was boron phosphate and vinylene carbonate, the mass of the boron phosphate was 1% of the total mass of the electrolyte, the mass of the vinylene carbonate was 1% of the total mass of the electrolyte.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), the additive was boron phosphate and vinyl ethylene carbonate, the mass of the boron phosphate was 1% of the total mass of the electrolyte, the mass of the vinyl ethylene carbonate was 1% of the total mass of the electrolyte.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), the additive was boron phosphate and maleic anhydride, the mass of the boron phosphate was 1% of the total mass of the electrolyte, the mass of the maleic anhydride was 1% of the total mass of the electrolyte.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), there was no additive in the electrolyte.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), the additive was boron phosphate, the mass of the boron phosphate was 0.001% of the total mass of the electrolyte.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), the additive was boron phosphate, the mass of the boron phosphate was 8% of the total mass of the electrolyte.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), the additive was ethylene sulfate, the mass of the ethylene sulfate was 1% of the total mass of the electrolyte.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), the additive was 1,3-propanesultone, the mass of the 1,3-propanesultone was 1% of the total mass of the electrolyte.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), the additive was vinylene carbonate, the mass of the vinylene carbonate was 1% of the total mass of the electrolyte.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), the additive was vinyl ethylene carbonate, the mass of the vinyl ethylene carbonate was 1% of the total mass of the electrolyte.
- the lithium-ion secondary battery was prepared according to example 1, except that in the preparation of the electrolyte (step (3)), the additive was maleic anhydride, the mass of the maleic anhydride was 1% of the total mass of the electrolyte.
- the lithium-ion secondary battery was charged to 4.2 V at a constant current of 1 C, then the lithium-ion secondary battery was charged to 0.05 C at a constant voltage of 4.2 V, then the lithium-ion secondary battery was discharged to 2.8 V at a constant current of 1 C, the obtained discharge capacity was the discharge capacity before the high temperature storage process of the lithium-ion secondary battery; then the lithium-ion secondary battery was charged to 4.2 V at a constant current of 1 C, then the lithium-ion secondary battery was stored for 30 days under 60° C., after the high temperature storage process was completed, the lithium-ion secondary battery was placed in the environment of 25° C., then the lithium-ion secondary battery was discharged to 2.8 V at a constant current of 0.5 C, then the lithium-ion secondary battery was charged to 4.2 V at a constant current of 1 C, then the lithium-ion secondary battery was charged to 0.05 C at a constant voltage of 4.2 V, then the lithium-ion secondary battery was discharged to 2.8 V
- Capacity retention rate after stored for 30 days under 60° C. of the lithium-ion secondary battery (%) (the discharge capacity after the high temperature storage process of the lithium-ion secondary battery/the discharge capacity before the high temperature storage process of the lithium-ion secondary battery) ⁇ 100%.
- the lithium-ion secondary battery was charged to 4.2 V at a constant current of 1 C, then the lithium-ion secondary battery was charged to 0.05 C at a constant voltage of 4.2 V, then the lithium-ion secondary battery was discharged to 2.8 V at a constant current of 1 C, then the lithium-ion secondary battery was charged to 4.2 V at a constant current of 1 C, then the lithium-ion secondary battery was charged to 0.05 C at a constant voltage of 4.2 V, the lithium-ion secondary battery was fully charged.
- the volume of the lithium-ion secondary battery was measured by using the drainage method and the measured volume was the volume before the high temperature storage process.
- volume expansion rate after stored for 30 days under 70° C. of the lithium-ion secondary battery (%) (the volume after the high temperature storage process/the volume before the high temperature storage process ⁇ 1) ⁇ 100%.
- the boron phosphate might inhibit the side reactions between the electrolyte and the positive active material when the lithium-ion secondary battery was used under high temperature environment, thereby improving the capacity retention rate after the high temperature cycle process and the capacity retention rate after the high temperature storage process of the lithium-ion secondary battery. Meanwhile, there was also a complexation reaction between the B atom in the boron phosphate and the hydrofluoric acid in the electrolyte, therefore the volume expansion rate after the high temperature storage process of the lithium-ion secondary battery was decreased.
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Abstract
Description
Capacity retention rate after 500 cycles under 60° C. of the lithium-ion secondary battery (%)=(discharge capacity of 500th cycle/discharge capacity of the first cycle)×100%.
Capacity retention rate after stored for 30 days under 60° C. of the lithium-ion secondary battery (%)=(the discharge capacity after the high temperature storage process of the lithium-ion secondary battery/the discharge capacity before the high temperature storage process of the lithium-ion secondary battery)×100%.
Volume expansion rate after stored for 30 days under 70° C. of the lithium-ion secondary battery (%)=(the volume after the high temperature storage process/the volume before the high temperature storage process−1)×100%.
TABLE 1 |
Parameters and test results of examples 1-9 and comparative examples 1-8 |
Capacity | Volume | ||||
Capacity | retention | expansion | |||
retention | rate after | rate after | |||
First additive | Second additive | rate after | stored for | stored for |
Mass | Mass | 500 cycles | 30 days | 30 days | ||||
percentage | percentage | under 60° C. | under 60° C. | under 70° C. | ||||
Type | (%) | Type | (%) | (%) | (%) | (%) | ||
Example 1 | Boron | 1 | / | / | 89 | 88 | 22 |
phosphate | |||||||
Example 2 | Boron | 0.5 | / | / | 87 | 86 | 25 |
phosphate | |||||||
Example 3 | Boron | 3 | / | / | 90 | 89 | 19 |
phosphate | |||||||
Example 4 | Boron | 5 | / | / | 92 | 91 | 18 |
phosphate | |||||||
Example 5 | Boron | 1 | Ethylene sulfate | 1 | 92 | 91 | 11 |
phosphate | |||||||
Example 6 | Boron | 1 | 1,3-propanesultone | 1 | 93 | 92 | 8 |
phosphate | |||||||
Example 7 | Boron | 1 | Vinylene carbonate | 1 | 92 | 91 | 11 |
phosphate | |||||||
Example 8 | Boron | 1 | Vinyl ethylene | 1 | 93 | 92 | 8 |
phosphate | carbonate | ||||||
Example 9 | Boron | 1 | Maleic anhydride | 1 | 92 | 93 | 9 |
phosphate | |||||||
Comparative | / | / | / | / | 78 | 79 | 35 |
example 1 | |||||||
Comparative | Boron | 0.001 | / | / | 79 | 80 | 34 |
example 2 | phosphate | ||||||
Comparative | Boron | 8 | / | / | 90 | 89 | 19 |
example 3 | phosphate | ||||||
Comparative | / | / | Ethylene sulfate | 1 | 89 | 88 | 16 |
example 4 | |||||||
Comparative | / | / | 1,3-propanesultone | 1 | 89 | 88 | 13 |
example 5 | |||||||
Comparative | / | / | Vinylene carbonate | 1 | 89 | 88 | 16 |
example 6 | |||||||
Comparative | / | / | Vinyl ethylene | 1 | 89 | 88 | 13 |
example 7 | carbonate | ||||||
Comparative | / | / | Maleic anhydride | 1 | 86 | 87 | 13 |
example 8 | |||||||
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